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Electrocatalytic reduction of NO to NH in ionic liquids by P-doped TiO nanotubes

《化学科学与工程前沿(英文)》 2023年 第17卷 第6期   页码 726-734 doi: 10.1007/s11705-022-2274-8

摘要: Designing advanced and cost-effective electrocatalytic system for nitric oxide (NO) reduction reaction (NORR) is vital for sustainable NH3 production and NO removal, yet it is a challenging task. Herein, it is shown that phosphorus (P)-doped titania (TiO2) nanotubes can be adopted as highly efficient catalyst for NORR. The catalyst demonstrates impressive performance in ionic liquid (IL)-based electrolyte with a remarkable high Faradaic efficiency of 89% and NH3 yield rate of 425 μg·h−1·mgcat.−1, being close to the best-reported results. Noteworthy, the obtained performance metrics are significantly larger than those for N2 reduction reaction. It also shows good durability with negligible activity decay even after 10 cycles. Theoretical simulations reveal that the introduction of P dopants tunes the electronic structure of Ti active sites, thereby enhancing the NO adsorption and facilitating the desorption of *NH3. Moreover, the utilization of IL further suppresses the competitive hydrogen evolution reaction. This study highlights the advantage of the catalyst−electrolyte engineering strategy for producing NH3 at a high efficiency and rate.

关键词: nitric oxide reduction reaction     electrcatalysis     ammonia production     phosphorus-doped titania    

Effects of support acidity on the reaction mechanisms of selective catalytic reduction of NO by CH

Shicheng XU, Junhua LI, Dong YANG, Jiming HAO

《环境科学与工程前沿(英文)》 2009年 第3卷 第2期   页码 186-193 doi: 10.1007/s11783-009-0016-5

摘要: The reaction mechanisms of selective catalytic reduction (SCR) of nitric oxide (NO) by methane (CH ) over solid superacid-based catalysts were proposed and testified by DRIFTS studies on transient reaction as well as by kinetic models. Catalysts derived from different supports would lead to different reaction pathways, and the acidity of solid superacid played an important role in determining the reaction mechanisms and the catalytic activities. Higher ratios of Br?nsted acid sites to Lewis acid sites would lead to stronger oxidation of methane and then could facilitate the step of methane activation. Strong Br?nsted acid sites would not necessarily lead to better catalytic performance, however, since the active surface NO species and the corresponding reaction routes were determined by the overall acidity strength of the support. The reaction routes where NO moiety was engaged as an important intermediate involved moderate oxidation of methane, the rate of which could determine the overall activity. The reaction involving NO moiety was likely to be determined by the step of reduction of NO. Therefore, to enhance the SCR activity of solid superacid catalysts, reactions between appropriate couples of active NO species and activated hydrocarbon intermediates should be realized by modification of the support acidity.

关键词: selective catalytic reduction (SCR)     nitric oxide (NO)     methane     support acidity     Br?nsted acid sites     NOy species    

EFFECTS OF TRANSPORT STRESS ON THE INTESTINES INVOLVING NEURONAL NITRIC OXIDE SYNTHASE

《农业科学与工程前沿(英文)》   页码 285-295 doi: 10.15302/J-FASE-2022469

摘要:

● Transport stress declined the level of leukocytes including lymphocytes in rat serum.

关键词: intestine     nNOS     nNOS-positive neurons     transport stress    

Expression of inducible nitric oxide synthase in trophoblasts and deciduas in early medical abortion

Geqing XIA, Chaoying WU

《医学前沿(英文)》 2009年 第3卷 第2期   页码 216-219 doi: 10.1007/s11684-009-0028-3

摘要: The purpose of this study was to investigate the expression of inducible nitric oxide synthase in trophoblasts and deciduas in early medical abortion, and study the relationship of medical abortion through mifepristone and inducible nitric oxide synthase (iNOS) in early pregnancy. Expression of iNOS in trophoblasts and deciduas was detected by both hybridization and immunohistochemical assay in 40 patients (experimental group); the positive expression of iNOS was represented by number density (N/S) and positive unit (Pu) using computer color magic image analysis system (CMIAS). All results were compared with that obtained from vacuum aspiration. In the experimental group, N/S and Pu in trophoblasts were 0.120 ± 0.010 and 15.3 ± 2.6, respectively, while in the control group, they were 0.021 ± 0.003 and 3.1 ± 0.5, respectively, and there were significant differences between the two groups. By immunohistochemical assay, N/S and Pu were 0.090 ± 0.010, 10.24 ± 1.55 0.016 ± 0.002, 1.26 ± 0.33 in the trophoblasts of the two groups; there were also significant differences between the two groups. There were lower iNOS expressions in deciduas by in situ hybridization and immunohistochemical assay, and the difference between the two groups was not significant.It was concluded that mifepristone induced medical abortion through the expression of iNOS in trophoblasts but not in deciduas.

关键词: mifepristone     inducible nitric oxide synthase     early pregnancy     placental immunity    

Role of nitric oxide in biological effects of vascular endothelial growth factor

Qigong LIU M D , Yan ZENG , Jiani LIU , Shan YE , Yongdong LI , Zaiying LU M D ,

《医学前沿(英文)》 2009年 第3卷 第3期   页码 284-286 doi: 10.1007/s11684-009-0062-1

摘要: To evaluate the role of nitric oxide in the biological effects of vascular endothelial growth factor (VEGF) and the possible mechanism of VEGF, the cultured vascular endothelial cells of rabbit aorta were divided into control group, VEGF-treated group and VEGF+ -nitro-L-arginine methyl ester (L-NAME)-treated group. The absorbance () value of vascular endothelial cells and the levels of prostaglandin (PGI), endothelin-1 (ET-1) and von Willebrand factor (vWF) in the supernatant were observed by water-soluble tetrazolium salt assay, radioimmunoassay and enzyme-linked immunosorbent assay. The values and PGI in VEGF-treated group and VEGF+L-NAME-treated group were higher than those in control group (<0.05 and <0.01). The ET-1 and vWF were significantly decreased in VEGF-treated group and VEGF+L-NAME-treated group compared with the control (<0.05 and <0.01). These results indicate that VEGF could promote the proliferation and secretion of PGI and inhibit the secretion of ET-1 and vWF in vascular endothelial cells and that L-NAME could inhibit the effect of VEGF partially. Nitric oxide is an important mediator in the process of stimulating proliferation and regulating secretion of vascular endothelial cells by VEGF.

关键词: vascular endothelial growth factor     nitric oxide     N-nitro-L-arginine methyl ester     vascular endothelial cells    

Effects of resistin on insulin signaling in endothelial cells

Zhizhen LI, Fangping LI, Jianhong YE, Li YAN, Zuzhi FU

《医学前沿(英文)》 2009年 第3卷 第2期   页码 136-140 doi: 10.1007/s11684-009-0029-2

摘要: The objective of this study was to investigate the effects of resistin on insulin signaling in human umbilical vein endothelial cells (HUVECs). HUVECs were incubated with recombinant human resistin (0-100 ng/mL) for 24 h. Akt and endothelial nitric oxide synthase (eNOS) phosphorylation levels of endothelial cells under basal or insulin stimulated conditions were measured by Western blot. Nitric oxide (NO) production of HUVECs was also detected. The results showed that resistin could significantly inhibit Akt and eNOS phosphorylation and NO production in endothelial cells under insulin stimulated conditions ( < 0.05 control). But under basal conditions, treatment with resistin could result in a decrease in eNOS phosphorylation ( < 0.05 control) but had no effect on NO production and Akt phosphorylation levels. These findings suggested that resistin exerted an inhibitory effect on NO production by inhibiting insulin signaling and eNOS phosphorylation in endothelial cells.

关键词: resistin     endothelium     nitric oxide     endothelial nitric oxide synthase     Akt-binding protein     mouse    

Relationship of endothelial nitric oxide synthase gene polymorphism with blood pressure, lipid profile

TANG Zhongzhi, LI Junyao, YANG Jianhong

《医学前沿(英文)》 2008年 第2卷 第2期   页码 178-181 doi: 10.1007/s11684-008-0033-y

摘要: To study the relationship of the polymorphism of endothelial nitric oxide synthase (eNOS) gene and blood pressure, lipid profiles and blood glucose level. By using PCR-RFLP, the eNOS Glu298Asp gene polymorphism was detected in 184 patients with essential hypertension and 196 matched healthy individuals with normal blood pressure. Taking into account eNOS Glu298Asp polymorphisms, the relationship of blood pressure with triglycerides (TG), total cholesterol (TC), high density lipoprotein (HDL), low density lipoprotein (LDL) and blood glucose level was analyzed. The distribution of eNOS Glu298Asp polymorphism had no significant difference between different blood pressure groups and gender groups, but there was a significant difference between different age groups, diastolic blood pressure groups or BMI groups ( < 0.05). Asp/Asp genotype significantly increased the risk of hypertension in individuals with serum TC above 5.4 mmol/L ( = 0.03, = 2.65). eNOS Glu298Asp polymorphism and serum lipid could synergistically modulate the blood pressure. eNOS Asp/Asp genotype could significantly increase the risk of hypertension in individuals with serum TC over 5.4 mmol/L. eNOS Glu298Asp in combination with serum TC could be used to predict the risk of hypertension.

Removal of nitric oxide from simulated flue gas using aqueous persulfate with activation of ferrous ethylenediaminetetraacetate

《化学科学与工程前沿(英文)》 2023年 第17卷 第4期   页码 460-469 doi: 10.1007/s11705-022-2224-5

摘要: Nitric oxide being a major gas pollutant has attracted much attention and various technologies have been developed to reduce NO emission to preserve the environment. Advanced persulfate oxidation technology is a workable and effective choice for wet flue gas denitrification due to its high efficiency and green advantages. However, NO absorption rate is limited and affected by mass transfer limitation of NO and aqueous persulfate in traditional reactors. In this study, a rotating packed bed (RPB) was employed as a gas–liquid absorption device to elevate the NO removal efficiency (ηNO) by aqueous persulfate ((NH4)2S2O8) activated by ferrous ethylenediaminetetraacetate (Fe2+-EDTA). The experimental results regarding the NO absorption were obtained by investigating the effect of various operating parameters on the removal efficiency of NO in RPB. Increasing the concentration of (NH4)2S2O8 and liquid–gas ratio could promoted the oxidation and absorption of NO while the ηNO decreased with the increase of the gas flow and NO concentration. In addition, improving the high gravity factor increased the ηNO and the total volumetric mass transfer coefficient (KGα) which raise the ηNO up to more than 75% under the investigated system. These observations proved that the RPB can enhance the gas–liquid mass transfer process in NO absorption. The correlation formula between KGα and the influencing factors was determined by regression calculation, which is used to guide the industrial scale-up application of the system in NO removal. The presence of O2 also had a negative effect on the NO removal process and through electron spin resonance spectrometer detection and product analysis, it was revealed that Fe2+-EDTA activated (NH4)2S2O8 to produce •SO4, •OH and •O2, played a leading role in the oxidation of NO, to produce NO3 as the final product. The obtained results demonstrated a good applicable potential of RPB/PS/Fe2+-EDTA in the removal of NO from flue gases.

关键词: rotating packed bed     Fe2+-EDTA     sulfate radical     hydroxyl radical     NO removal efficiency    

Photocatalytic reduction of carbon dioxide by titanium oxide-based semiconductors to produce fuels

Xi CHEN, Fangming JIN

《能源前沿(英文)》 2019年 第13卷 第2期   页码 207-220 doi: 10.1007/s11708-019-0628-9

摘要: To tackle the crisis of global warming, it is imperative to control and mitigate the atmospheric carbon dioxide level. Photocatalytic reduction of carbon dioxide into solar fuels furnishes a gratifying solution to utilize and reduce carbon dioxide emission and simultaneously generate renewable energy to sustain the societies. So far, titanium oxide-based semiconductors have been the most prevalently adopted catalysts in carbon dioxide photoreduction. This mini-review provides a general summary of the recent progresses in titanium oxide-catalyzed photocatalytic reduction of carbon dioxide. It first illustrates the use of structural engineering as a strategy to adjust and improve the catalytic performances. Then, it describes the introduction of one/two exogenous elements to modify the photocatalytic activity and/or selectivity. Lastly, it discusses multi-component hybrid titanium oxide composites.

关键词: photocatalysis     carbon dioxide reduction     semiconductors     titanium oxide     renewable fuels    

Heterometallic cluster-based organic frameworks as highly active electrocatalysts for oxygen reductionand oxygen evolution reaction: a density functional theory study

《化学科学与工程前沿(英文)》 2023年 第17卷 第5期   页码 570-580 doi: 10.1007/s11705-022-2247-y

摘要: Recently, metal–organic frameworks are one of the potential catalytic materials for electrocatalytic applications. The oxygen reduction reaction and oxygen evolution reaction catalytic activities of heterometallic cluster-based organic frameworks are investigated using density functional theory. Firstly, the catalytic activities of heterometallic clusters are investigated. Among all heterometallic clusters, Fe2Mn–Mn has a minimum overpotential of 0.35 V for oxygen reduction reaction, and Fe2Co–Co possesses the smallest overpotential of 0.32 V for oxygen evolution reaction, respectively 100 and 50 mV lower than those of Pt(111) and RuO2(110) catalysts. The analysis of the potential gap of Fe2M clusters indicates that Fe2Mn, Fe2Co, and Fe2Ni clusters possess good bifunctional catalytic activity. Additionally, the catalytic activity of Fe2Mn and Fe2Co connected through 3,3′,5,5′-azobenzenetetracarboxylate linker to form Fe2M–PCN–Fe2M is explored. Compared with Fe2Mn–PCN–Fe2Mn, Fe2Co–PCN–Fe2Co, and isolated Fe2M clusters, the mixed-metal Fe2Co–PCN–Fe2Mn possesses excellent bifunctional catalytic activity, and the values of potential gap on the Mn and Co sites of Fe2Co–PCN–Fe2Mn are 0.69 and 0.70 V, respectively. Furthermore, the analysis of the electron structure indicates that constructing a mixed-metal cluster can efficiently enhance the electronic properties of the catalyst. In conclusion, the mixed-metal cluster strategy provides a new approach to further design and synthesize high-efficiency bifunctional electrocatalysts.

关键词: bimetallic metal–organic frameworks     bifunctional electrocatalyst     density functional theory     oxygen reduction reaction     oxygen evolution reaction    

Recent advances and challenges of nitrogen/nitrate electro catalytic reduction to ammonia synthesis

《能源前沿(英文)》 doi: 10.1007/s11708-023-0908-2

摘要: The Haber-Bosch process is the most widely used synthetic ammonia technology at present. Since its invention, it has provided an important guarantee for global food security. However, the traditional Haber-Bosch ammonia synthesis process consumes a lot of energy and causes serious environmental pollution. Under the serious pressure of energy and environment, a green, clean, and sustainable ammonia synthesis route is urgently needed. Electrochemical synthesis of ammonia is a green and mild new method for preparing ammonia, which can directly convert nitrogen or nitrate into ammonia using electricity driven by solar, wind, or water energy, without greenhouse gas and toxic gas emissions. Herein, the basic mechanism of the nitrogen reduction reaction (NRR) to ammonia and nitrate reduction reaction (NO3 RR) to ammonia were discussed. The representative approaches and major technologies, such as lithium mediated electrolysis and solid oxide electrolysis cell (SOEC) electrolysis for NRR, high activity catalyst and advanced electrochemical device fabrication for NO3 RR and electrochemical ammonia synthesis were summarized. Based on the above discussion and analysis, the main challenges and development directions for electrochemical ammonia synthesis were further proposed.

关键词: electrochemical ammonia synthesis     nitrogen     nitrate     nitrogen reduction reaction (NRR) to ammonia     nitrate reduction reaction (NO–3 RR)    

Nitrous oxide formation and emission in selective non-catalytic reduction process

YANG Weijuan, ZHOU Junhu, ZHOU Zhijun, CEN Kefa

《能源前沿(英文)》 2007年 第1卷 第2期   页码 228-232 doi: 10.1007/s11708-007-0031-9

摘要: Pulverized coal-fired boilers are not nitrous oxide sources because of high temperature combustion. But selective non-catalytic reduction may produce NO by NO reduction reactions. Chemical kinetics calculation and experimental research were used to find out the mechanism between NO and N-agent species, N-agent/NO nitrogen stoichiometric ratio (NSR), reaction temperature, reaction time, etc. The results show that NO emission decreases with increasing reaction temperature and NSR decreases when reaction time is enough. NO concentration first increases then decreases as SNCR reactions keep on occuring. Ammonia SNCR tests indicated that NO emission was 0 7 μmol/mol. About 8.7% of NO was transformed to NO, and NO emission was 27.8 μmol/mol at urea-SNCR test. Urea-SNCR is likely to bring NO emission problem.

Reduction of CeO

Elena Yu. KONYSHEVA

《化学科学与工程前沿(英文)》 2013年 第7卷 第3期   页码 249-261 doi: 10.1007/s11705-013-1333-6

摘要: Reduction behavior of pure and doped CeO , the multi-phase La Sr CoO ? CeO , La Sr MnO ? CeO , and La Ni Fe O ? CeO composites, was studied under hydrogen containing atmosphere to address issues related to the improvement of electrochemical and catalytic performance of electrodes in fuel cells. The enhanced reduction of cerium oxide was observed initially at 800°C in all composites in spite of the presence of highly reducible transition metal cations that could lead to the increase in surface concentration of oxygen vacancies and generation of the electron enriched surface. Due to continuous reduction of cerium oxide in La Sr CoO ? CeO and La Sr MnO ? CeO (up to 10 h) composites the redox activity of the Ce /Ce pair could be suppressed and additional measures are required for reversible spontaneous regeneration of Ce . After 3 h exposure to H -Ar at 800°C the reduction of cerium oxides and perovskite phases in La Ni Fe O ? CeO composites was diminished. The extent of cerium oxide involvement in the reduction process varies with time, and depends on its initial deviation from oxygen stoichiometry (that results in the larger lattice parameter and the longer pathway for O transport through the fluorite lattice), chemical origin of transition metal cations in the perovskite, and phase diversity in multi-phase composites.

关键词: reduction of cerium oxide     composites     perovskites     catalyst under hydrogen containing atmosphere    

Isolation of microbe for asymmetric reduction of prochiral aromatic ketone and its reaction characters

YANG Zhonghua, WANG Yu, WANG Guanghui, ZENG Rong, YAO Shanjing

《化学科学与工程前沿(英文)》 2007年 第1卷 第4期   页码 416-420 doi: 10.1007/s11705-007-0076-7

摘要: The favorable microbes for the asymmetric reduction of prochiral aromatic ketones was isolated from soil using acetophenone as the sole carbon source, when the asymmetric reduction of acetophenone (ACP) to chiral ?-phenethyl alcohol (PEA) was chosen as the model reaction. Two microbe strains with excellent catalytic activity were obtained. They were and identified by bacteria identification. The product of the asymmetric reduction of ACP catalyzed by was mainly R-PEA and that by was mainly S-PEA. The yield and enantiomeric excesses (e.e.) could respectively reach 75% and 90% for , and 80% and 70% for , much higher than those catalyzed by baker s yeast.

关键词: excellent catalytic     prochiral aromatic     enantiomeric     -phenethyl     catalytic activity    

Numerical investigation of the chemical and electrochemical characteristics of planar solid oxide fuel

Yuzhang WANG, Shilie WENG, Yiwu WENG

《能源前沿(英文)》 2011年 第5卷 第2期   页码 195-206 doi: 10.1007/s11708-011-0148-8

摘要: A fully three-dimensional mathematical model of a planar solid oxide fuel cell (SOFC) with complete direct internal steam reforming was constructed to investigate the chemical and electrochemical characteristics of the porous-electrode-supported (PES)-SOFC developed by the Central Research Institute of Electric Power Industry of Japan. The effective kinetic models developed over the Ni/YSZ anode takes into account the heat transfer and species diffusion limitations in this porous anode. The models were used to simulate the methane steam reforming processes at the co- and counter-flow patterns. The results show that the flow patterns of gas and air have certain effects on cell performance. The cell at the counter-flow has a higher output voltage and output power density at the same operating conditions. At the counter-flow, however, a high hotspot temperature is observed in the anode with a non-fixed position, even when the air inlet flow rate is increased. This is disadvantageous to the cell. Both cell voltage and power density decrease with increased air flow rate.

关键词: planar solid oxide fuel cell (SOFC)     direct internal reforming     chemical reaction     methane     electrochemical    

标题 作者 时间 类型 操作

Electrocatalytic reduction of NO to NH in ionic liquids by P-doped TiO nanotubes

期刊论文

Effects of support acidity on the reaction mechanisms of selective catalytic reduction of NO by CH

Shicheng XU, Junhua LI, Dong YANG, Jiming HAO

期刊论文

EFFECTS OF TRANSPORT STRESS ON THE INTESTINES INVOLVING NEURONAL NITRIC OXIDE SYNTHASE

期刊论文

Expression of inducible nitric oxide synthase in trophoblasts and deciduas in early medical abortion

Geqing XIA, Chaoying WU

期刊论文

Role of nitric oxide in biological effects of vascular endothelial growth factor

Qigong LIU M D , Yan ZENG , Jiani LIU , Shan YE , Yongdong LI , Zaiying LU M D ,

期刊论文

Effects of resistin on insulin signaling in endothelial cells

Zhizhen LI, Fangping LI, Jianhong YE, Li YAN, Zuzhi FU

期刊论文

Relationship of endothelial nitric oxide synthase gene polymorphism with blood pressure, lipid profile

TANG Zhongzhi, LI Junyao, YANG Jianhong

期刊论文

Removal of nitric oxide from simulated flue gas using aqueous persulfate with activation of ferrous ethylenediaminetetraacetate

期刊论文

Photocatalytic reduction of carbon dioxide by titanium oxide-based semiconductors to produce fuels

Xi CHEN, Fangming JIN

期刊论文

Heterometallic cluster-based organic frameworks as highly active electrocatalysts for oxygen reductionand oxygen evolution reaction: a density functional theory study

期刊论文

Recent advances and challenges of nitrogen/nitrate electro catalytic reduction to ammonia synthesis

期刊论文

Nitrous oxide formation and emission in selective non-catalytic reduction process

YANG Weijuan, ZHOU Junhu, ZHOU Zhijun, CEN Kefa

期刊论文

Reduction of CeO

Elena Yu. KONYSHEVA

期刊论文

Isolation of microbe for asymmetric reduction of prochiral aromatic ketone and its reaction characters

YANG Zhonghua, WANG Yu, WANG Guanghui, ZENG Rong, YAO Shanjing

期刊论文

Numerical investigation of the chemical and electrochemical characteristics of planar solid oxide fuel

Yuzhang WANG, Shilie WENG, Yiwu WENG

期刊论文